arXiv subjects

Paul G. Evans

Publications and source records attributed to Paul G. Evans.

At least 19 recordsLinked to original sources

arXiv2026

Terahertz oscillation of $180^{\circ}$ domain walls in ferroelectric membranes

A fundamentally intriguing yet not well understood topic in the field of ferroelectrics is the collective excitation of domain walls (DWs), with potential applications to DW-based nanoelectronic and optoelectronic devices. Here we use dynamical phase-field simulations to identify the collective modes of an Ising-type $180^{\circ}$ DW in a uniaxially strained BaTiO3 membrane. The membrane, which concurrently functions as a cavity for polarization and acoustic waves, permits cavity-enhanced resonant excitation of polarization waves. The simulation reveals an unconventional DW sliding mode that exhibits a bulk-polarization-charge-driven nonzero resonant frequency in the sub-terahertz (THz) regime with a dynamically changing internal structure during sliding. These features differ from the previously reported zero-frequency DW sliding mode or the surface-polarization-charge-driven DW sliding mode. The effect of strain on the frequency of this unconventional DW sliding mode and other previously known THz DW eigenmodes is investigated by dynamical phase-field simulations and interpreted by eigenmode analysis or analytical calculation in a simplified one-dimensional (1D) system. These results provide new insights into the high-frequency dynamics of ferroelectric DWs and suggest opportunities for realizing strain control of phonon-DW resonance, and more broadly, for discovering and controlling unconventional DW modes in conventional domain patterns with applications to reconfigurable THz and optical devices.

cond-mat.mtrl-sci↗

arXiv2024

High-resolution spatio-temporal strain imaging reveals loss mechanisms in a surface acoustic wave device

Surface acoustic wave devices are key components for processing radio frequency signals in wireless communication because these devices offer simultaneously high performance, compact size and low cost. The optimization of the device structure requires a quantitative understanding of energy conversion and loss mechanisms. Stroboscopic full-field diffraction x-ray microscopy studies of a prototypical one-port resonator device revealed the existence of unanticipated acoustic loss. A non-uniform acoustic excitation in the active area was responsible for the substantial end and side leakages observed at the design frequency. Quantitative analysis of the strain amplitude using a wave decomposition method allowed the determination of several key device parameters. This high-resolution spatiotemporal strain imaging technique is, more generally, suited for studying nanophononics, specifically when the feature size is smaller than optical wavelengths. The strain sensitivity allows precise measurement of acoustic waves with picometer-scale amplitude.

physics.app-ph↗

arXiv2024

Resolving Length Scale Dependent Transient Disorder Through an Ultrafast Phase Transition

Material functionality can be strongly determined by structure extending only over nanoscale distances. The pair distribution function presents an opportunity to shift structural studies beyond idealized crystal models and investigate structure over varying length scales. Applying this method with ultrafast time resolution has the potential to similarly disrupt the study of structural dynamics and phase transitions. Here, we demonstrate such a measurement of CuIr$_{2}$S$_{4}$ optically pumped from its low temperature Ir-dimerized phase. Dimers are optically suppressed without spatial correlation, generating a structure whose level of disorder depends strongly on length scale. The re-development of structural ordering over tens of picoseconds is directly tracked over both space and time as a transient state is approached. This measurement demonstrates both the crucial role of local structure and disorder in non-equilibrium processes and the feasibility of accessing this information with state-of-the-art XFEL facilities.

cond-mat.mtrl-sci↗

arXiv2024

Hybrid magnon-phonon cavity for large-amplitude terahertz spin-wave excitation

Terahertz (THz) spin waves or their quanta, magnons, can be efficiently excited by acoustic phonons because these excitations have similar wavevectors in the THz regime. THz acoustic phonons can be produced using photoacoustic phenomena but typically have a low population and thus a relatively low displacement amplitude. The magnetization amplitude and population of the acoustically excited THz magnons are thus usually small. Using analytical calculations and dynamical phase-field simulations, we show that a freestanding metal/magnetic-insulator (MI)/dielectric multilayer can be designed to produce large-amplitude THz spin wave via cavity-enhanced magnon-phonon interaction. The amplitude of the acoustically excited THz spin wave in the freestanding multilayer is predicted to be more than ten times larger than in a substrate-supported multilayer. Acoustically excited nonlinear magnon-magnon interaction is demonstrated in the freestanding multilayer. The simulations also indicate that the magnon modes can be detected by probing the charge current in the metal layer generated via spin-charge conversion across the MI/metal interface and the resulting THz radiation. Applications of the freestanding multilayer in THz optoelectronic transduction are computationally demonstrated.

cond-mat.mes-hall↗

arXiv2023

Detection Sensitivity Limit of Hundreds of Atoms with X-Ray Fluorescence Microscopy

We report X-ray fluorescence (XRF) imaging of nanoscale inclusions of impurities for quantum technology. A very bright diffraction-limited focus of the X-ray beam produces very high sensitivity and resolution. We investigated gallium (Ga) dopants in silicon (Si) produced by a focused ion beam (FIB). These dopants might provide 3/2-spin qubits or p-type electrical contacts and quantum dots. We find that the ion beam spot is somewhat larger than expected, and the technique provides a useful calibration for the resolution of FIBs. Enticingly, we demonstrate that with a single shot detection of 1 second integration time, the sensitivity of the XRF would be sufficient to find amongst background a single isolated inclusion of unknown location comprising only 3000 Ga impurities (a mass of just 350 zg) without any need for specialized nm-thickness lamellae, and down from >105 atoms in previous reports of similar work. With increased integration we were able to detect 650 impurities. The results show that planned facility upgrades might achieve single atom sensitivity with a generally applicable, non-destructive technique in the near future.

cond-mat.mtrl-sci↗

arXiv2022

Optically Induced Picosecond Lattice Compression in the Dielectric Component of a Strongly Coupled Ferroelectric/Dielectric Superlattice

Above-bandgap femtosecond optical excitation of a ferroelectric/dielectric BaTiO3/CaTiO3 superlattice leads to structural responses that are a consequence of the screening of the strong electrostatic coupling between the component layers. Time-resolved x-ray free-electron laser diffraction shows that the structural response to optical excitation includes a net lattice expansion of the superlattice consistent with depolarization-field screening driven by the photoexcited charge carriers. The depolarization-field-screening-driven expansion is separate from a photoacoustic pulse launched from the bottom electrode on which the superlattice was epitaxially grown. The distribution of diffracted intensity of superlattice x-ray reflections indicates that the depolarization-field-screening-induced strain includes a photoinduced expansion in the ferroelectric BaTiO3 and a contraction in CaTiO3. The magnitude of expansion in BaTiO3 layers is larger than the contraction in CaTiO3. The difference in the magnitude of depolarization-field-screening-driven strain in the BaTiO3 and CaTiO3 components can arise from the contribution of the oxygen octahedral rotation patterns at the BaTiO3/CaTiO3 interfaces to the polarization of CaTiO3. The depolarization-field-screening-driven polarization reduction in the CaTiO3 layers points to a new direction for the manipulation of polarization in the component layers of a strongly coupled ferroelectric/dielectric superlattice.

cond-mat.mtrl-sci↗

arXiv2022

Dynamic Tilting of Ferroelectric Domain Walls via Optically Induced Electronic Screening

Optical excitation perturbs the balance of phenomena selecting the tilt orientation of domain walls within ferroelectric thin films. The high carrier density induced in a low-strain BaTiO3 thin film by an above-bandgap ultrafast optical pulse changes the tilt angle that 90° a/c domain walls form with respect to the substrate-film interface. The dynamics of the changes are apparent in time-resolved synchrotron x-ray scattering studies of the domain diffuse scattering. Tilting occurs at 298 K, a temperature at which the a/b and a/c domain phases coexist but is absent at 343 K in the better ordered single-phase a/c regime. Phase coexistence at 298 K leads to increased domain-wall charge density, and thus a larger screening effect than in the single-phase regime. The screening mechanism points to new directions for the manipulation of nanoscale ferroelectricity.

cond-mat.mtrl-sci↗

arXiv2022

Low-temperature nanoscale heat transport in a gadolinium iron garnet heterostructure probed by ultrafast x-ray diffraction

Time-resolved x-ray diffraction has been used to measure the low-temperature thermal transport properties of a Pt/Gd3Fe5O12//Gd3Ga5O12 metal/oxide heterostructure relevant to applications in spin caloritronics. A pulsed femtosecond optical signal produces a rapid temperature rise in the Pt layer, followed by heat transport into the Gd3Fe5O12 (GdIG) thin film and the Gd3Ga5O12 (GGG) substrate. The time dependence of x-ray diffraction from the GdIG layer was tracked using an accelerator-based femtosecond x-ray source. The ultrafast diffraction measurements probed the intensity of the GdIG (1 -1 2) x-ray reflection in a grazing-incidence x-ray diffraction geometry. The comparison of the variation of the diffracted x-ray intensity with a model including heat transport and the temperature dependence of the GdIG lattice parameter allows the thermal conductance of the Pt/GdIG and GdIG//GGG interfaces to be determined. Complementary synchrotron x-ray diffraction studies of the low-temperature thermal expansion properties of the GdIG layer provide a precise calibration of the temperature dependence of the GdIG lattice parameter. The interfacial thermal conductance of the Pt/GdIG and GdIG//GGG interfaces determined from the time-resolved diffraction study is of the same order of magnitude as previous reports for metal/oxide and epitaxial dielectric interfaces. The thermal parameters of the Pt/GdIG//GGG heterostructure will aid in the design and implementation of thermal transport devices and nanostructures.

cond-mat.mtrl-sci↗

arXiv2021

Solid phase epitaxial growth of the correlated-electron transparent conducting oxide SrVO3

SrVO3 thin films with a high figure of merit for applications as transparent conductors were crystallized from amorphous layers using solid phase epitaxy (SPE). Epitaxial SrVO3 films crystallized on SrTiO3 using SPE exhibit a room temperature resistivity of 2.5 x 10-5 Ohms cm, a residual resistivity ratio of 3.8, and visible light transmission above 0.5 for a 60 nm-thick film. SrVO3 layers were deposited at room temperature using radio-frequency sputtering in an amorphous form and subsequently crystallized by heating in controlled gas environment. The lattice parameters and mosaic angular width of x-ray reflections from the crystallized films are consistent with partial relaxation of the strain resulting from the epitaxial mismatch between SrVO3 and SrTiO3. A reflection high-energy electron diffraction study of the kinetics of SPE indicates that crystallization occurs via the thermally activated propagation of the crystalline/amorphous interface, similar to SPE phenomena in other perovskite oxides. Thermodynamic calculations based on density functional theory predict the temperature and oxygen partial pressure conditions required to produce the SrVO3 phase and are consistent with the experiments. The separate control of deposition and crystallization conditions in SPE presents new possibilities for the crystallization of transparent conductors in complex geometries and over large areas.

cond-mat.mtrl-sci↗

arXiv2021

Structural evidence for ultrafast polarization rotation in ferroelectric/dielectric superlattice nanodomains

Weakly coupled ferroelectric/dielectric superlattice thin film heterostructures exhibit complex nanoscale polarization configurations that arise from a balance of competing electrostatic, elastic, and domain-wall contributions to the free energy. A key feature of these configurations is that the polarization can locally have a significant component that is not along the thin-film surface normal direction, while maintaining zero net in-plane polarization. PbTiO3/SrTiO3 thin-film superlattice heterostructures on a conducting SrRuO3 bottom electrode on SrTiO3 have a room-temperature stripe nanodomain pattern with nanometer-scale lateral period. Ultrafast time-resolved x-ray free electron laser diffraction and scattering experiments reveal that above-bandgap optical pulses induce rapidly propagating acoustic pulses and a perturbation of the domain diffuse scattering intensity arising from the nanoscale stripe domain configuration. With 400 nm optical excitation, two separate acoustic pulses are observed: a high-amplitude pulse resulting from strong optical absorption in the bottom electrode and a weaker pulse arising from the depolarization field screening effect due to absorption directly within the superlattice. The picosecond scale variation of the nanodomain diffuse scattering intensity is consistent with a larger polarization change than would be expected due to the polarization-tetragonality coupling of uniformly polarized ferroelectrics. The polarization change is consistent instead with polarization rotation facilitated by the reorientation of the in-plane component of the polarization at the domain boundaries of the striped polarization structure. The complex steady-state configuration within these ferroelectric heterostructures leads to polarization rotation phenomena that have been previously available only through the selection of bulk crystal composition.

cond-mat.mtrl-sci↗

arXiv2021

Subterahertz collective dynamics of polar vortices

The collective dynamics of topological structures have been of great interest from both fundamental and applied perspectives. For example, the studies of dynamical properties of magnetic vortices and skyrmions not only deepened the understanding of many-body physics but also led to potential applications in data processing and storage. Topological structures constructed from electrical polarization rather than spin have recently been realized in ferroelectric superlattices, promising for ultrafast electric-field control of topological orders. However, little is known about the dynamics of such complex extended nanostructures which in turn underlies their functionalities. Using terahertz-field excitation and femtosecond x-ray diffraction measurements, we observe ultrafast collective polarization dynamics that are unique to polar vortices, with orders of magnitude higher frequencies and smaller lateral size than those of experimentally realized magnetic vortices. A previously unseen soft mode, hereafter referred to as a vortexon, emerges as transient arrays of nanoscale circular patterns of atomic displacements, which reverse their vorticity on picosecond time scales. Its frequency is significantly reduced at a critical strain, indicating a condensation of structural dynamics. First-principles-based atomistic calculations and phase-field modeling reveal the microscopic atomic arrangements and frequencies of the vortex modes. The discovery of subterahertz collective dynamics in polar vortices opens up opportunities for applications of electric-field driven data processing in topological structures with ultrahigh speed and density.

cond-mat.mes-hall↗

arXiv2020

Instrument for in situ hard x-ray nanobeam characterization during epitaxial crystallization and materials transformations

Solid-phase epitaxy (SPE) and other three-dimensional epitaxial crystallization processes pose challenging structural and chemical characterization problems. The concentration of defects, the spatial distribution of elastic strain, and the chemical state of ions each vary with nanoscale characteristic length scales and depend sensitively on the gas environment and elastic boundary conditions during growth. The lateral or three-dimensional propagation of crystalline interfaces in SPE has nanoscale or submicron characteristic distances during typical crystallization times. An in situ synchrotron hard x-ray instrument allows these features to be studied during deposition and crystallization using diffraction, resonant scattering, nanobeam and coherent diffraction imaging, and reflectivity. The instrument incorporates a compact deposition system allowing the use of short-working-distance x-ray focusing optics. Layers are deposited using radio-frequency magnetron sputtering and evaporation sources. The deposition system provides control of the gas atmosphere and sample temperature. The sample is positioned using a stable mechanical design to minimize vibration and drift and employs precise translation stages to enable nanobeam experiments. Results of in situ x-ray characterization of the amorphous thin film deposition process for a SrTiO3/BaTiO3 multilayer illustrate implementation of this instrument.

cond-mat.mtrl-sci↗

arXiv2020

Mesoscopic Elastic Distortions in GaAs Quantum Dot Heterostructures

Quantum devices formed in high-electron-mobility semiconductor heterostructures provide a route through which quantum mechanical effects can be exploited on length scales accessible to lithography and integrated electronics. The electrostatic definition of quantum dots in semiconductor heterostructure devices intrinsically involves the lithographic fabrication of intricate patterns of metallic electrodes. The formation of metal/semiconductor interfaces, growth processes associated with polycrystalline metallic layers, and differential thermal expansion produce elastic distortion in the active areas of quantum devices. Understanding and controlling these distortions presents a significant challenge in quantum device development. We report synchrotron x-ray nanodiffraction measurements combined with dynamical x-ray diffraction modeling that reveal lattice tilts with a depth-averaged value up to 0.04 deg. and strain on the order of 10^-4 in the two-dimensional electron gas (2DEG) in a GaAs/AlGaAs heterostructure. Elastic distortions in GaAs/AlGaAs heterostructures modify the potential energy landscape in the 2DEG due to the generation of a deformation potential and an electric field through the piezoelectric effect. The stress induced by metal electrodes directly impacts the ability to control the positions of the potential minima where quantum dots form and the coupling between neighboring quantum dots.

cond-mat.mes-hall↗

arXiv2020

Three-dimensional phonon population anisotropy in silicon nanomembranes

Nanoscale single-crystals possess modified phonon dispersions due to the truncation of the crystal. The introduction of surfaces alters the population of phonons relative to the bulk and introduces anisotropy arising from the breaking of translational symmetry. Such modifications exist throughout the Brillouin zone, even in structures with dimensions of several nanometers, posing a challenge to the characterization of vibrational properties and leading to uncertainty in predicting the thermal, optical, and electronic properties of nanomaterials. Synchrotron x-ray thermal diffuse scattering studies find that freestanding Si nanomembranes with thicknesses as large as 21 nm exhibit a higher scattering intensity per unit thickness than bulk silicon. In addition, the anisotropy arising from the finite thickness of these membranes produces particularly intense scattering along reciprocal-space directions normal to the membrane surface compared to corresponding in-plane directions. These results reveal the dimensions at which calculations of materials properties and device characteristics based on bulk phonon dispersions require consideration of the nanoscale size of the crystal.

cond-mat.mes-hall↗

arXiv2019

Role of temperature-dependent electron trapping dynamics in the optically driven nanodomain transformation in a PbTiO${_3}$/SrTiO${_3}$ superlattice

The spontaneously formed striped polarization nanodomain configuration of a PbTiO${_3}$/SrTiO${_3}$ superlattice transforms to a uniform polarization state under above-bandgap illumination with a time dependence varying with the intensity of optical illumination and a well-defined threshold intensity. Recovery after the end of illumination occurs over a temperature-dependent period of tens of seconds at room temperature and shorter times at elevated temperatures. A model in which the screening of the depolarization field depends on the population of trapped electrons correctly predicts the observed temperature and optical intensity dependence.

cond-mat.mtrl-sci↗

arXiv2019

Non-thermal fluence threshold for femtosecond pulsed x-ray radiation damage in perovskite complex oxide epitaxial heterostructures

Intense hard x-ray pulses from a free-electron laser induce irreversible structural damage in a perovskite oxide epitaxial heterostructure when pulse fluences exceed a threshold value. The intensity of x-ray diffraction from a 25-nm thick epitaxial BiFeO$_{3}$ layer on a SrTiO$_{3}$ substrate measured using a series of pulses decreases abruptly with a per-pulse fluence of 2.7 x 10$^{6}$ photons $μ$m$^{-2}$ at 9.7 keV photon energy, but remains constant for 1.3 x 10$^{6}$ photons $μ$m$^{-2}$ or less. The damage resulted in the destruction of the BiFeO$_{3}$ thin film within the focal spot area and the formation of a deep cavity penetrating into the STO substrate via the removal of tens of nanometers of material per pulse. The damage threshold occurs at a fluence that is insufficient to heat the absorption volume to the melting point. The morphology of the ablated sample is consistent with fracture rather than melting. Together these results indicate that the damage occurs via a non-thermal process consistent with ultrafast ionization of the absorption volume.

cond-mat.mtrl-sci↗

arXiv2019

Nanosecond Optically Induced Phase Transformation in Compressively Strained BiFeO3 on LaAlO3

Above-bandgap optical illumination induces a transformation from tilted tetragonal-like (T-like) and rhombohedral-like (R-like) phases to an untilted T-like phase in compressively strained BiFeO3. Optical excitation leads to an out-of-plane lattice expansion in the T-like phase. The transformation proceeds in regions with boundaries between the T-like and tilted R-like and tilted T-like phases, consistent with the motion of a boundary. The optically induced transformation indicates that there are new optically driven routes towards nanosecond-scale control of phase transformations in ferroelectrics and multiferroics.

cond-mat.mes-hall↗

arXiv2017

Photoinduced Domain Pattern Transformation in Ferroelectric/Dielectric Superlattices

The nanodomain pattern in ferroelectric/dielectric superlattices transforms to a uniform polarization state under above-bandgap optical excitation. X-ray scattering reveals a disappearance of domain diffuse scattering and an expansion of the lattice. The reappearance of the domain pattern occurs over a period of seconds at room temperature, suggesting a transformation mechanism in which charge carriers in long-lived trap states screen the depolarization field. A Landau-Ginzburg-Devonshire model predicts changes in lattice parameter and a critical carrier concentration for the transformation.

cond-mat.mtrl-sci↗